High-voltage spinel manganese oxide LiNi0.5Mn1.5O4 (LNMO) that possesses high energy densities, high thermal and electrochemical stabilities, good operating safeties, low costs, and good rate performance has been well recognized to have great potential for power batteries. Despite these merits, unqualified electrolytes are still a big obstacle toward mass production of LNMO-based lithium-ion batteries (LIBs). To address this obstacle, solid polymer electrolytes (SPEs) have been increasingly considered as promising candidates thus far. Here, we mainly discuss the inherent advantages and ideal requirements of SPEs coupling with LNMO cathodes and then systematically review the recent advances of SPEs from the perspective of structure–performance relationships for the first time. Finally, prospects and challenges of the SPE systems are also discussed. This Review aims to guide rational structure design and future development of state-of-the-art SPEs with high anodic stabilities, boosting the practical applications of high-voltage LNMO cathode-based LIBs.

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High voltage spinel manganese oxide LiNi0.5Mn1.5O4 (LNMO) cathodes are promising for practical applications owing to several strengths including high working voltages, excellent operating safety, low costs, and so on. However, LNMO-based lithium–ion batteries (LIBs) fade rapidly mainly owing to unqualified electrolytes, hence becoming a big obstacle toward practical applications. To tackle this roadblock, substantial progress has been made thus far, and yet challenges still remain, while rare reviews have systematically discussed the status quo and future development of electrolyte optimization coupling with LNMO cathodes. Here, we discuss cycling degradation mechanisms at the cathode/electrolyte interface and ideal requirements of electrolytes for LNMO cathode-equipped LIBs, as well as review the recent advance of electrolyte optimization for LNMO cathode-equipped LIBs in detail. And then, the perspectives regarding the future research opportunities in developing state-of-the-art electrolytes are also presented. The authors hope to shed light on the rational optimization of advanced organic electrolytes in order to boost the large-scale practical applications of high voltage LNMO cathode-based LIBs.

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By virtue of environmental friendliness, low cost, and the high theoretical capacity of sulfur (1675 mAh/g), metal–sulfur batteries (MSBs), as promising next-generation rechargeable cells, have attracted ever-increasing attention from both academic and industrial fields. Despite good progress, however, thus far MSBs have been rarely able to bring their energy storage performance up to the needed levels of reliability due to challenging issues such as the shuttle effect of polysulfides, low utilization efficiency of the S, inferior cycling performance, and safety hazards. To tackle this, the rational optimization of the electrolyte, which tremendously affects the cycling stability, rate capability, lifespan, and safety of the investigated batteries, is considered to be one of the crucial directions to improve the performance of MSBs. Herein we outline the challenges and recent optimization progress on electrolytes in MSBs with Li, Na, Mg, Ca, K, and Al as metal anodes. The topics regarding the fundamentals of electrolyte optimization strategies and the possible solution to further performance improvement are highlighted. Finally, a perspective on further electrolyte development is presented. This discussion aims at gaining good insight into the rational design of electrolytes so as to boost the commercial process of MSB development.

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Incompatible interphases resulting from the irreconcilable contradiction between impedance and mechanical strength have become one of the major obstacles to the practical application of solid-state lithium metal batteries (SSLMBs). With the employment of a decoupling strategy by rational topological design, herein a topological polymer-reinforced interphase layer is in situ constructed using a synthesized solid polymer electrolyte. As a result, the constructed topological solid electrolyte interphase (SEI) layer harmonizes the enhanced mechanochemical stability and fast diffusion dynamics of Li + , which maintains the integrity and stability of the SEI layer during cycling. In addition, a highly stable and reversible Li nucleation/stripping behaviors exceeding 3000 h and the superior cycling performance of practical LiFePO 4 /Li metal battery beyond 500 cycles can be achieved by virtue of the formation of the topological interphase layer. This design strategy of constructing a topological interphase layer to decouple mechanical strength and the activation energy of Li + transport provides a feasible paradigm for realizing practical SSLMBs.